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[Katsuhiko Ariga](https://orcid.org/0000-0002-2445-2955)

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Materials Nanoarchitectonics for Advanced DevicesCitation: Ariga, K. MaterialsNanoarchitectonics for AdvancedDevices. Materials 2024, 17, 5918.https://doi.org/10.3390/ma17235918Academic Editors: VlassiosLikodimos and Daniela KovachevaReceived: 28 October 2024Revised: 19 November 2024Accepted: 2 December 2024Published: 3 December 2024Copyright: © 2024 by the author.Licensee MDPI, Basel, Switzerland.This article is an open access articledistributed under the terms andconditions of the Creative CommonsAttribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).ReviewMaterials Nanoarchitectonics for Advanced DevicesKatsuhiko Ariga 1,21 Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS),1-1 Namiki, Tsukuba 305-0044, Ibaraki, Japan; ariga.katsuhiko@nims.go.jp2 Graduate School of Frontier Sciences, The University of Tokyo, 5-1-5 Kashiwanoha,Kashiwa 277-8561, Chiba, JapanAbstract: Advances in nanotechnology have made it possible to observe and evaluate structuresdown to the atomic and molecular level. The next step in the development of functional materials is toapply the knowledge of nanotechnology to materials sciences. This is the role of nanoarchitectonics,which is a concept of post-nanotechnology. Nanoarchitectonics is defined as a methodology tocreate functional materials using nanounits such as atoms, molecules, and nanomaterials as buildingblocks. Nanoarchitectonics is very general and is not limited to materials or applications, and thusnanoarchitecture is applied in many fields. In particular, in the evolution from nanotechnology tonanoarchitecture, it is useful to consider the contribution of nanoarchitecture in device applications.There may be a solution to the widely recognized problem of integrating top-down and bottom-upapproaches in the design of functional systems. With this in mind, this review discusses examplesof nanoarchitectonics in developments of advanced devices. Some recent examples are introducedthrough broadly dividing them into organic molecular nanoarchitectonics and inorganic materialsnanoarchitectonics. Examples of organic molecular nanoarchitecture include a variety of controlstructural elements, such as π-conjugated structures, chemical structures of complex ligands, sterichindrance effects, molecular stacking, isomerization and color changes due to external stimuli,selective control of redox reactions, and doping control of organic semiconductors by electrontransfer reactions. Supramolecular chemical processes such as association and intercalation of organicmolecules are also important in controlling device properties. The nanoarchitectonics of inorganicmaterials often allows for control of size, dimension, and shape, and their associated physicalproperties can also be controlled. In addition, there are specific groups of materials that are suitablefor practical use, such as nanoparticles and graphene. Therefore, nanoarchitecture of inorganicmaterials also has a more practical aspect. Based on these aspects, this review finally considers thefuture of materials nanoarchitectonics for further advanced devices.Keywords: nanoarchitectonics; advanced device; doping control of organic semiconductor; inorganicmaterials nanoarchitectonics; organic molecular nanoarchitectonics; structural control1. IntroductionThe global community is confronted with a multitude of challenges, including thoserelated to energy [1–7], the environment [8–14], medicine [15–21], and information [22–28].The development of functional materials represents a crucial step in addressing thesechallenges and paving the way for a more sustainable future. It is imperative that materialsbe developed which are capable of meeting a multitude of demands through the utilizationof a diverse array of material chemistries. In this context, it is crucial to regulate thenanostructure of functional materials. The internal nanostructure of a given materialcan vary significantly, resulting in notable differences in the material’s properties andfunctions [29–33]. An increase in the interfacial area and optimization of the relativearrangement of each component can result in a significant improvement in functionalefficiency [34–38]. The advent of nanotechnology has served to reinforce the importanceof these nanostructures. Advances in nanotechnology have enabled the observation ofMaterials 2024, 17, 5918. https://doi.org/10.3390/ma17235918 https://www.mdpi.com/journal/materialshttps://doi.org/10.3390/ma17235918https://doi.org/10.3390/ma17235918https://creativecommons.org/https://creativecommons.org/licenses/by/4.0/https://creativecommons.org/licenses/by/4.0/https://www.mdpi.com/journal/materialshttps://www.mdpi.comhttps://orcid.org/0000-0002-2445-2955https://doi.org/10.3390/ma17235918https://www.mdpi.com/journal/materialshttps://www.mdpi.com/article/10.3390/ma17235918?type=check_update&version=1Materials 2024, 17, 5918 2 of 27structures at the atomic and molecular levels [39–43]. Furthermore, the physical propertiesof such nanostructures and nanospaces have been elucidated [44–48]. The subsequentphase in the advancement of functional materials is to integrate the insights derived fromnanotechnology into the material development process. In other words, it is to reconsiderfunctional materials using nanounits, including atoms, molecules, and nanoparticles. Thisis the responsibility of nanoarchitectonics, which is a concept of post-nanotechnology [49].Similarly, the concept of nanotechnology was first proposed by Richard Feynman in the mid-20th century [50,51], and nanoarchitectonics was subsequently introduced by MasakazuAono in the early 21st century [52,53].Nanoarchitectonics is the concept of constructing functional material systems fromthe fundamental building blocks of atoms, molecules, and nanomaterials (Figure 1). Inthis process, a combination of atom and molecule manipulation, chemical transforma-tion (such as organic synthesis), physical material transformation, self-assembly and self-organization, arrangement and orientation by external fields and forces, nano- and micro-fabrication technology, and biochemical processes are employed [54,55]. The creation offunctional structures and the conversion of molecules into materials have also been subjectsof extensive studies in past histories. The processes of self-assembly in supramolecularchemistry [56–60], metal–organic frameworks (MOFs) by coordination chemistry [61–65],covalent organic frameworks (COFs) by polymer chemistry [66–70], and template synthe-sis in materials science [71–75] all serve functions similar in parts to nanoarchitectonics.Furthermore, self-assembled monolayers (SAMs) [76–80], the Langmuir–Blodgett (LB)method [81–85], and layer-by-layer (LbL) assembly [86–90], which combine molecularassemblies and interface science technology, have also been often employed. In fact, theyexhibit a pronounced nanoarchitectonics character. Therefore, nanoarchitectonics does notrepresent an entirely novel field of inquiry; rather, it offers an integrated conceptual frame-work that encompasses nanotechnology and a wide range of materials sciences [91,92].As evidenced by the preceding background description, nanoarchitectonics is a highlygeneral concept that can be applied without being limited to specific materials or appli-cations. All materials are composed of atoms and molecules. Consequently, the conceptof nanoarchitectonics, which constructs functional materials from units such as atomsand molecules, may be regarded as the ultimate methodology that can be applied to allmaterials. In analogy with the theory of everything [93], which represents the ultimate goalof physics, nanoarchitectonics may be considered a method for everything in materialsscience [94,95].The increasing prevalence of nanoarchitectonics in a diverse array of fields is alsoevidenced by the growing number of publications that utilize the term “nanoarchitec-tonics” in their paper titles. The aforementioned papers span a diverse range of disci-plines, encompassing material synthesis [96–102], structural control [103–109], the investi-gation of physical phenomena [110–116], fundamental biochemistry [117–123], chemicalcatalysis [124–130], photocatalysis [131–137], solar cells [138–144], fuel cells [145–151],various batteries [152–158], supercapacitors [159–165], and other energy-related applica-tions [166–172]. The concept of nanoarchitectonics is also being employed in a number ofpractical fields, including environmental purification [173–179], biosensors [180–186], drugdelivery [187–193], tissue engineering [194–200], and biomedicine [201–207]. Furthermore,the concept of nanoarchitectonics is being employed in the integration of artificial structureswith organic, bio, and nanomaterials, as evidenced by its use in the sensor [208–214] anddevice fields [215–221].Indeed, it can be argued that device technology has been a significant beneficiary of theadvancements in nanotechnology. Significant progress has been made in the precise struc-tural aspects of device development due to the advancement of various microfabricationtechnologies and the evaluation of nanostructures. In the context of nanoarchitectonics, it isvaluable to consider the role of nanotechnology in the development of device applications.This may provide a solution to the widely recognized problem of integrating top-downand bottom-up approaches in functional system development [222–224]. This is becauseMaterials 2024, 17, 5918 3 of 27microfabrication technology, which has been a highly influential force in nanotechnology,is a representative example of a top-down approach. In contrast, nanoarchitectonics, whichinvolves the construction of functional materials from the atomic and molecular levels, is apowerful bottom-up approach. Device nanoarchitectonics will represent the convergenceof the top-down and bottom-up approaches that have been identified as being essential. Itwill serve as an exemplar of the convergence of nanotechnology and materials science.Materials 2024, 17, x FOR PEER REVIEW 3 of 27   top-down and bottom-up approaches in functional system development [222–224]. This is because microfabrication technology, which has been a highly influential force in nan-otechnology, is a representative example of a top-down approach. In contrast, nanoarchi-tectonics, which involves the construction of functional materials from the atomic and molecular levels, is a powerful bottom-up approach. Device nanoarchitectonics will rep-resent the convergence of the top-down and bottom-up approaches that have been iden-tified as being essential. It will serve as an exemplar of the convergence of nanotechnology and materials science.  Figure 1. Nanoarchitectonics as the concept of constructing functional material systems from the fundamental building blocks of atoms, molecules, and nanomaterials (from the top) and device nanoarchitectonics as the convergence of the top-down and bottom-up approaches (bottom) [54,95]. In light of the aforementioned context, this review will examine a number of exam-ples pertaining to nanoarchitectonics as it relates to devices. This review presents a Figure 1. Nanoarchitectonics as the concept of constructing functional material systems from thefundamental building blocks of atoms, molecules, and nanomaterials (from the top) and devicenanoarchitectonics as the convergence of the top-down and bottom-up approaches (bottom) [54,95].In light of the aforementioned context, this review will examine a number of examplespertaining to nanoarchitectonics as it relates to devices. This review presents a selection ofrecent publications on devices with the term “nanoarchitectonics” in their title, in orderto figure out the realistic effects of nanoarchitectonics. Therefore, the described topics donot cover all the existing science and technology. Furthermore, this review also introducesMaterials 2024, 17, 5918 4 of 27other device papers that incorporate aspects of nanoarchitectonics. The following sectionpresents the aforementioned papers, which have been roughly categorized into two distinctgroups: organic molecular nanoarchitectonics and inorganic materials nanoarchitectonics.It should be noted that this selection does not represent a comprehensive overview of allrelevant examples. However, it is believed to reflect trends and characteristics. Based onthese considerations, this review also contemplates the prospective evolution of materialsnanoarchitectonics in the context of advanced devices.2. Organic Molecular NanoarchitectonicsThe construction of these devices is based on microfabrication technology. However,the characteristics of the devices are contingent upon the materials from which they areconstructed in nanoscale. The functionality of devices that exhibit optical or electroniccharacteristics is contingent upon the properties of the molecules that perform thosefunctions. In other words, the development of functional molecules represents a significantchallenge and potential breakthrough. If we consider the development of functionalmolecules as an effort to create and assemble basic molecules, it can be said that this is theresult of molecular nanoarchitectonics. In particular, organic molecular nanoarchitectonics,which encompasses the design and synthesis of organic molecules, represents a significantfactor in the development of devices. The following section will present a number ofexamples that align with this concept and will examine the key elements involved.Rigid, planar carbon nanostructures with extended π-conjugation represent an attrac-tive option for the development of nanoarchitectonics-based devices. They are notable fortheir distinctive properties, including high carrier mobility, robust absorption and emissionin the long wavelength region, and the material properties of molecular assemblies, whichare influenced by the control of intermolecular interactions in the condensed state. One ofthe factors that determines these functional properties is the mode and extent of π-extension.The development of functional molecules exhibiting unique photophysical and electronicproperties can be achieved through the appropriate chemical and structural modificationsof molecular nanoarchitectonics. Acenes have been the subject of considerable attentionas a class of linearly π-extended polycyclic aromatic hydrocarbons that exhibit promisingthin-film organic field-effect transistor performance. Murai, Takai, and colleagues havereported the nanoarchitectonics of introducing azulene into linear π-extended polycyclicaromatic hydrocarbons (Figure 2) [225]. Azulenes are a class of polycyclic aromatic hydro-carbons that have the potential to be utilized as linear π-extended structural isomers ofpentacene and picene. New derivatives with two symmetrically fused azulene rings weresynthesized in order to further elucidate the effect of incorporating the azulene ring. Itwas discovered that the gap between the highest occupied molecular orbital (HOMO) andthe lowest unoccupied molecular orbital (LUMO) (HOMO–LUMO gap) can be reducedto a level comparable to that of [n]acene. Additionally, the researchers observed that thecompounds exhibited high stability against air under visible light, with a narrow HOMO–LUMO gap comparable to that of pentacene. In accordance with this HOMO–LUMOgap, the absorption band exhibited a red shift. An X-ray single-crystal structure analysisrevealed that the five fused azulene rings adopted a herringbone-packing structure, whichis the result of a balance of CH–π and π–π interactions. Organic field-effect transistors werefabricated in a bottom-gate/bottom-contact configuration, utilizing a 400 nm thick SiO2layer as the gate dielectric. This novel derivative comprising azulene rings was synthesizedvia thermal deposition under high vacuum conditions. The transfer and output curves ofthe thin-film organic field-effect transistors exhibited the expected behavior for a normallyoff field-effect transistor. The fabrication of organic field-effect transistor devices with thisderivative resulted in the observation of typical p-type behavior. The results indicate thatthe molecular nanoarchitectonics of fusing azulene to carbon and heterocycles may be avaluable approach for designing devices with specific electronic and photophysical proper-ties. In particular, the potential of this derivative as a new class of p-type semiconductorwas clearly demonstrated.Materials 2024, 17, 5918 5 of 27Materials 2024, 17, x FOR PEER REVIEW 5 of 27   azulene to carbon and heterocycles may be a valuable approach for designing devices with specific electronic and photophysical properties. In particular, the potential of this deriv-ative as a new class of p-type semiconductor was clearly demonstrated.  Figure 2. Nanoarchitectonics of introducing azulene into linear π-extended polycyclic aromatic hy-drocarbons where the gap between HOMO and LUMO can be reduced to a level comparable to that of [n]acene. Reprinted with permission from [225]. Copyright 2023 Oxford University Press. Stable deep-red organic light-emitting devices (OLEDs) have the potential to serve as a distinctive source of illumination for plant growth and health monitoring systems. Nev-ertheless, the electron-to-photon conversion efficiency, expressed as external quantum ef-ficiency, is markedly inferior to that of other primary colors. One promising strategy to enhance the external quantum efficiency of stable deep-red OLEDs is the utilization of exciplex host systems. Sasabe, Kido, and colleagues developed n-type exciplex host part-ners based on quinoline-modified phenanthroline derivatives [226]. The HOMO, LUMO, and triplet energy of the relevant molecules were estimated (Figure 3). The calculated tri-plet energy values were markedly larger, indicating the effective confinement of triplet excitons in the emitter. The developed derivatives formed exciplexes in combination with the p-type host material N,N′-di-1-naphthyl-N,N′-diphenylbenzidine, which was em-ployed as the host material for deep-red phosphorescent OLEDs. The devices exhibited low turn-on voltages and high current density and brightness. This can be attributed to the excellent electron injection properties of these derivatives, which are caused by their higher electron affinity value. Furthermore, it demonstrates the most optimal performance among deep-red phosphorescent OLEDs. With regard to thermal stability, the material demonstrated high thermal stability with a glass transition temperature of up to 148 °C. This evidence supports the assertion that phenanthroline derivatives are promising n-type host materials. It is anticipated that this will facilitate the expeditious development and commercialization of n-type semiconductors and promote their utilization as distinctive lighting sources for plant growth and health monitoring systems. Figure 2. Nanoarchitectonics of introducing azulene into linear π-extended polycyclic aromatichydrocarbons where the gap between HOMO and LUMO can be reduced to a level comparable tothat of [n]acene. Reprinted with permission from [225]. Copyright 2023 Oxford University Press.Stable deep-red organic light-emitting devices (OLEDs) have the potential to serveas a distinctive source of illumination for plant growth and health monitoring systems.Nevertheless, the electron-to-photon conversion efficiency, expressed as external quantumefficiency, is markedly inferior to that of other primary colors. One promising strategyto enhance the external quantum efficiency of stable deep-red OLEDs is the utilization ofexciplex host systems. Sasabe, Kido, and colleagues developed n-type exciplex host partnersbased on quinoline-modified phenanthroline derivatives [226]. The HOMO, LUMO, andtriplet energy of the relevant molecules were estimated (Figure 3). The calculated tripletenergy values were markedly larger, indicating the effective confinement of triplet excitonsin the emitter. The developed derivatives formed exciplexes in combination with the p-typehost material N,N′-di-1-naphthyl-N,N′-diphenylbenzidine, which was employed as thehost material for deep-red phosphorescent OLEDs. The devices exhibited low turn-onvoltages and high current density and brightness. This can be attributed to the excellentelectron injection properties of these derivatives, which are caused by their higher electronaffinity value. Furthermore, it demonstrates the most optimal performance among deep-redphosphorescent OLEDs. With regard to thermal stability, the material demonstrated highthermal stability with a glass transition temperature of up to 148 ◦C. This evidence supportsthe assertion that phenanthroline derivatives are promising n-type host materials. It isanticipated that this will facilitate the expeditious development and commercializationof n-type semiconductors and promote their utilization as distinctive lighting sources forplant growth and health monitoring systems.Thermally activated delayed fluorescence emitters based on widely available metalelements will emerge as the most promising contenders for the next generation of or-ganic light-emitting diodes (OLEDs). Sasabe and colleagues developed a mononuclearAl complex with a β-diketone ligand that exhibited excellent thermally activated delayedfluorescence properties (Figure 4) [227]. In order to enhance the optical functions of thepreviously used molecules, molecular nanoarchitectonics was employed to modify thechemical structure of the β-diketone ligand by the addition of a donor unit. The utilizationof this β-diketone derivative resulted in a notable enhancement of the photoluminescencequantum yield of the emitter, while the metal complexation led to a considerable improve-ment in the optical functions of the original diketone ligand in the solid state. The opticalMaterials 2024, 17, 5918 6 of 27functional advantages of this complex include a very high photoluminescence quantumyield, a rapid radiative decay rate, and a short delayed fluorescence lifetime in the solidstate. DFT calculations demonstrated that metal complexation could generate a distinctiveelectronic structure, which could markedly enhance the optical functions of the originaldiketone ligand. The application of nanoarchitectonics to organic light-emitting devicesresults in the attainment of high external quantum efficiency and low turn-on voltage,which are advantageous for the realization of low-power-consumption devices.Materials 2024, 17, x FOR PEER REVIEW 6 of 27    Figure 3. n-type exciplex host partners based on quinoline-modified phenanthroline derivatives with estimation of HOMO and LUMO, where the calculated triplet energy values were markedly larger, indicating effective confinement of triplet excitons in the emitter. Reprinted with permission from [226]. Copyright 2023 Oxford University Press. Thermally activated delayed fluorescence emitters based on widely available metal elements will emerge as the most promising contenders for the next generation of organic light-emitting diodes (OLEDs). Sasabe and colleagues developed a mononuclear Al com-plex with a β-diketone ligand that exhibited excellent thermally activated delayed fluo-rescence properties (Figure 4) [227]. In order to enhance the optical functions of the previ-ously used molecules, molecular nanoarchitectonics was employed to modify the chemi-cal structure of the β-diketone ligand by the addition of a donor unit. The utilization of this β-diketone derivative resulted in a notable enhancement of the photoluminescence quantum yield of the emitter, while the metal complexation led to a considerable improve-ment in the optical functions of the original diketone ligand in the solid state. The optical functional advantages of this complex include a very high photoluminescence quantum yield, a rapid radiative decay rate, and a short delayed fluorescence lifetime in the solid state. DFT calculations demonstrated that metal complexation could generate a distinctive electronic structure, which could markedly enhance the optical functions of the original diketone ligand. The application of nanoarchitectonics to organic light-emitting devices results in the attainment of high external quantum efficiency and low turn-on voltage, which are advantageous for the realization of low-power-consumption devices. Figure 3. n-type exciplex host partners based on quinoline-modified phenanthroline derivativeswith estimation of HOMO and LUMO, where the calculated triplet energy values were markedlylarger, indicating effective confinement of triplet excitons in the emitter. Reprinted with permissionfrom [226]. Copyright 2023 Oxford University Press.Ultrathin two-dimensional organic nanosheets exhibiting high mobility at a thicknessof a few molecular layers will demonstrate enhanced device performance. In particular, thedevelopment of ultrathin 2D organic nanosheets that simultaneously exhibit high lumines-cence efficiency and flexibility is a highly desirable objective. In a study titled “Hierarchicalnanoarchitectonics of ultrathin 2D organic nanosheets,” Zhang, Xie, and colleagues haveachieved the nanoarchitectonics of ultrathin 2D organic nanosheets (thickness: 19 nm) withdenser molecular packing [228]. In this component molecule, the orthogonal spirofluoreneexanthene scaffold exerts an efficient steric hindrance effect on intermolecular repulsion(Figure 5). Concurrently, the methoxyl and diphenylamine groups facilitate intermolecularattraction as supramolecular segments. π-π stacking and CH···π interactions reinforceantiparallel and interpenetrating molecular packing in dimeric aggregates with proximateintermolecular distances. These molecular nanoarchitectonics are conducive to the forma-tion of ultrathin 2D organic nanosheets. The restriction of conformational vibrations androtations may serve to minimize non-radiative deactivation in the solid state. By employinga self-assembly method, Zhang et al. [228] have successfully fabricated ultrathin 2D organicnanosheets with a thickness of approximately 19 nm in aqueous media, despite the tightmolecular packing. The ultrathin organic nanosheets can be molded into large, continuousmacroscale films via a one-step drop-coating method. The organic nanosheets displaysufficient flexibility. Even when the molecular stacking was denser, the ultrathin organicMaterials 2024, 17, 5918 7 of 27nanosheets prevented aggregation quenching and exhibited higher blue emission quantumyields than the amorphous films. These ultrathin 2D organic nanosheets may prove to bevaluable tools for the development of flexible electrically pumped lasers and intelligentquantum tunneling systems.Materials 2024, 17, x FOR PEER REVIEW 7 of 27    Figure 4. A mononuclear Al complex with a β-diketone ligand with excellent thermally activated delayed fluorescence properties. DFT calculations demonstrated that metal complexation could generate a distinctive electronic structure, which could markedly enhance the optical functions of the original diketone ligand. Reprinted with permission from [227]. Copyright 2023 Oxford Univer-sity Press. Ultrathin two-dimensional organic nanosheets exhibiting high mobility at a thick-ness of a few molecular layers will demonstrate enhanced device performance. In partic-ular, the development of ultrathin 2D organic nanosheets that simultaneously exhibit high luminescence efficiency and flexibility is a highly desirable objective. In a study titled “Hi-erarchical nanoarchitectonics of ultrathin 2D organic nanosheets,” Zhang, Xie, and col-leagues have achieved the nanoarchitectonics of ultrathin 2D organic nanosheets (thick-ness: 19 nm) with denser molecular packing [228]. In this component molecule, the or-thogonal spirofluorene exanthene scaffold exerts an efficient steric hindrance effect on in-termolecular repulsion (Figure 5). Concurrently, the methoxyl and diphenylamine groups facilitate intermolecular attraction as supramolecular segments. π-π stacking and CH···π interactions reinforce antiparallel and interpenetrating molecular packing in dimeric ag-gregates with proximate intermolecular distances. These molecular nanoarchitectonics are conducive to the formation of ultrathin 2D organic nanosheets. The restriction of confor-mational vibrations and rotations may serve to minimize non-radiative deactivation in the solid state. By employing a self-assembly method, Zhang et al. [228] have successfully fabricated ultrathin 2D organic nanosheets with a thickness of approximately 19 nm in aqueous media, despite the tight molecular packing. The ultrathin organic nanosheets can be molded into large, continuous macroscale films via a one-step drop-coating method. The organic nanosheets display sufficient flexibility. Even when the molecular stacking was denser, the ultrathin organic nanosheets prevented aggregation quenching and ex-hibited higher blue emission quantum yields than the amorphous films. These ultrathin 2D organic nanosheets may prove to be valuable tools for the development of flexible elec-trically pumped lasers and intelligent quantum tunneling systems. Figure 4. A mononuclear Al complex with a β-diketone ligand with excellent thermally activateddelayed fluorescence properties. DFT calculations demonstrated that metal complexation couldgenerate a distinctive electronic structure, which could markedly enhance the optical functionsof the original diketone ligand. Reprinted with permission from [227]. Copyright 2023 OxfordUniversity Press.Organic/polymer resistive random-access memory (RRAM) will constitute a pivotalcomponent in the field of bio-inspired electronics. It is anticipated that this technologywill find applications in advanced information storage, intelligent perception, brain-likesystems, and logic computing. Conversely, the capacity to expeditiously erase sensitivedata serves to bolster both information security and intellectual property protection. He,Wang, Chen, and colleagues synthesized polyvinyl spiropyran-grafted polydopamine-encapsulated structures for transient digital memristors (Figure 6) [229]. Indeed, blackphosphorus quantum dots functionalized with photochromic polyvinyl spiropyran-graftedpolydopamine are employed in the construction of transient digital memristors. The film,situated between ITO electrodes, was erased rapidly by UV irradiation within six seconds.Furthermore, the film exhibited typical nonvolatile digital memristor performance whensubjected to visible light irradiation. Upon UV irradiation, the closed-ring spiropyran formof the active layer is rapidly converted to the open-ring merocyanine form by “closed-to-open” isomerization, thereby enabling the information stored in the device to be rapidlyand completely erased. Furthermore, the potential of this memristor for handwritten digitrecognition was explored. A basic convolutional neural network comprising a convolu-tional layer and a pooling layer for filtering, and a fully connected layer for classification,was constructed. Following 10 epochs of training, the accuracy of digit recognition reached96.21%.In recent years, electrochromic devices have been employed in a multitude of applica-tions, including those pertaining to energy conservation and display technology. Never-theless, the advancement of lightweight, low-power, cost-effective, and environmentallybenign electrochromic devices remains a pivotal objective. In their study, entitled “A facilenanoarchitectonics of electrochromic devices”, Kim, You, and colleagues developed a novelelectrochromic device through the use of simple solution-cast polymerization [230]. In thisMaterials 2024, 17, 5918 8 of 27instance, the researchers employed a poly(3,4-ethylenedioxythiophene) (PEDOT)/2,2,6,6-tetramethylpiperidine-1-oxy-oxidized cellulose nanofiber epoxy composite. The fabricatedelectrochromic device exhibited a reversible color transition between light blue (translucentstate) and dark blue (colored state), dependent on the redox potential. This device isanticipated to provide a straightforward fabrication method for a range of energy-savingsmart windows and high-contrast displays.Materials 2024, 17, x FOR PEER REVIEW 8 of 27    Figure 5. Nanoarchitectonics of ultrathin 2D organic nanosheets with denser molecular packing: (top) the component molecule with the orthogonal spirofluorene exanthene scaffold; (bottom) the formation of ultrathin 2D organic nanosheets with its AFM image and its molecular-packing model. Reprinted with permission from [228]. Copyright 2023 Wiley-VCH. Organic/polymer resistive random-access memory (RRAM) will constitute a pivotal component in the field of bio-inspired electronics. It is anticipated that this technology will find applications in advanced information storage, intelligent perception, brain-like systems, and logic computing. Conversely, the capacity to expeditiously erase sensitive data serves to bolster both information security and intellectual property protection. He, Wang, Chen, and colleagues synthesized polyvinyl spiropyran-grafted polydopamine-en-capsulated structures for transient digital memristors (Figure 6) [229]. Indeed, black phos-phorus quantum dots functionalized with photochromic polyvinyl spiropyran-grafted polydopamine are employed in the construction of transient digital memristors. The film, situated between ITO electrodes, was erased rapidly by UV irradiation within six seconds. Furthermore, the film exhibited typical nonvolatile digital memristor performance when subjected to visible light irradiation. Upon UV irradiation, the closed-ring spiropyran form of the active layer is rapidly converted to the open-ring merocyanine form by “closed-to-open” isomerization, thereby enabling the information stored in the device to be rapidly and completely erased. Furthermore, the potential of this memristor for hand-written digit recognition was explored. A basic convolutional neural network comprising a convolutional layer and a pooling layer for filtering, and a fully connected layer for clas-sification, was constructed. Following 10 epochs of training, the accuracy of digit recogni-tion reached 96.21%. Figure 5. Nanoarchitectonics of ultrathin 2D organic nanosheets with denser molecular packing:(top) the component molecule with the orthogonal spirofluorene exanthene scaffold; (bottom) theformation of ultrathin 2D organic nanosheets with its AFM image and its molecular-packing model.Reprinted with permission from [228]. Copyright 2023 Wiley-VCH.The efficient storage and transport of electrical energy is a fundamental requirementfor the promotion of renewable energy-based electricity. Yamauchi and colleagues havedemonstrated an energy cycle based on a highly selective redox reaction between lactate andpyruvate, which are liquid at room temperature and obtained from biomass resources [231].The objective of their system is to achieve a completely low-emission outcome. An energystorage device, namely a lactic acid electrosynthesis cell (LAEC), was constructed for theproduction of lactate from pyruvate. This was achieved using a membrane electrode assem-bly (MEA), comprising a TiO2 cathode catalyst for the electroreduction of pyruvate andan IrOx anode catalyst for the oxidation of water (Figure 7A). The LAEC was constructedusing iridium oxide nanoparticles as the anode catalyst. The LAEC exhibits completesuppression of the hydrogen evolution reaction even in highly acidic aqueous solutions.Additionally, a direct lactic acid fuel cell (DLAFC) was constructed (Figure 7B). The directlactic acid fuel cell (DLAFC) employed platinum/cobalt and platinum–ruthenium/cobaltcatalysts as the cathode and anode catalysts, respectively. The DLAFC, utilizing 1 M lac-tate, demonstrated a selective oxidation of lactate to pyruvate. The combination of highlyMaterials 2024, 17, 5918 9 of 27selective electrochemical reactions in the LAEC and DLAFC allows for the direct storage ofelectrical energy in a biological liquid carrier. It is possible to complete a carbon-neutralenergy cycle using the resulting energy. The LAEC/DLAFC system has the advantageof being compact with low energy consumption, as it does not require high-temperatureconversion above 100 ◦C or the treatment of gaseous carriers.Materials 2024, 17, x FOR PEER REVIEW 9 of 27    Figure 6. Polyvinyl spiropyran-grafted polydopamine-encapsulated structures for transient digital memristors where black phosphorus quantum dots functionalized with photochromic polyvinyl spiropyran-grafted polydopamine are employed in the construction. Reprinted with permission from [229]. Copyright 2024 Oxford University Press. In recent years, electrochromic devices have been employed in a multitude of appli-cations, including those pertaining to energy conservation and display technology. Nev-ertheless, the advancement of lightweight, low-power, cost-effective, and environmen-tally benign electrochromic devices remains a pivotal objective. In their study, entitled “A facile nanoarchitectonics of electrochromic devices”, Kim, You, and colleagues developed a novel electrochromic device through the use of simple solution-cast polymerization [230]. In this instance, the researchers employed a poly(3,4-ethylenedioxythiophene) (PE-DOT)/2,2,6,6-tetramethylpiperidine-1-oxy-oxidized cellulose nanofiber epoxy composite. The fabricated electrochromic device exhibited a reversible color transition between light blue (translucent state) and dark blue (colored state), dependent on the redox potential. This device is anticipated to provide a straightforward fabrication method for a range of energy-saving smart windows and high-contrast displays. The efficient storage and transport of electrical energy is a fundamental requirement for the promotion of renewable energy-based electricity. Yamauchi and colleagues have demonstrated an energy cycle based on a highly selective redox reaction between lactate and pyruvate, which are liquid at room temperature and obtained from biomass resources [231]. The objective of their system is to achieve a completely low-emission outcome. An energy storage device, namely a lactic acid electrosynthesis cell (LAEC), was constructed for the production of lactate from pyruvate. This was achieved using a membrane elec-trode assembly (MEA), comprising a TiO₂ cathode catalyst for the electroreduction of py-ruvate and an IrOx anode catalyst for the oxidation of water (Figure 7A). The LAEC was constructed using iridium oxide nanoparticles as the anode catalyst. The LAEC exhibits complete suppression of the hydrogen evolution reaction even in highly acidic aqueous Figure 6. Polyvinyl spiropyran-grafted polydopamine-encapsulated structures for transient digitalmemristors where black phosphorus quantum dots functionalized with photochromic polyvinylspiropyran-grafted polydopamine are employed in the construction. Reprinted with permissionfrom [229]. Copyright 2024 Oxford University Press.It has been proposed that ultrathin polymer organic semiconductor films have a mul-titude of potential applications, including the development of flexible electronic devices.Nevertheless, in comparison to single crystals of low-molecular-weight organic semicon-ductors, there is considerable scope for further research in the areas of fabrication andproperty control. One illustrative example is the control of the electronic properties ofpolymer organic semiconductor films by doping. Ishii, Yamashita, and colleagues haverecently published a new study which demonstrates a novel coupling between proton-coupled electron transfer reactions, which are widely employed in biochemical processesand polymer organic semiconductors (Figure 8) [232]. A p-type organic semiconductorfilm was immersed in an aqueous solution containing a proton-coupled electron transferreaction redox couple (benzoquinone/hydroquinone) and a hydrophobic molecular ion.The redox potential of the former can be controlled by the proton activity (pH), which is aneasily manipulable parameter. The presence of p-type doping was confirmed by measuringthe absorption spectrum and conductivity. The efficient doping of polymer organic semi-conductor films is achieved through a synergistic reaction between proton-coupled electrontransfer reactions and the insertion of hydrophobic ions. The doping level was meticulouslyregulated within a pH-controlled aqueous solution. In other words, the Nernst equationMaterials 2024, 17, 5918 10 of 27was employed to regulate the Fermi level of the polymeric organic semiconductor thinfilm through the manipulation of proton activity. This doping method is also innovative inthat it can be performed in an aqueous solution at room temperature and pressure, whichrenders it a method that will also be useful for industrial applications. This could provebeneficial in the creation of a platform for room-temperature semiconductor processes andbiomolecular electronics. It will be feasible to establish a correlation between semiconductordoping and any chemical or biochemical process that can be linked with proton activity.This method is also regarded as a promising platform for biomolecular electronics.Materials 2024, 17, x FOR PEER REVIEW 10 of 27   solutions. Additionally, a direct lactic acid fuel cell (DLAFC) was constructed (Figure 7B). The direct lactic acid fuel cell (DLAFC) employed platinum/cobalt and platinum–ruthe-nium/cobalt catalysts as the cathode and anode catalysts, respectively. The DLAFC, uti-lizing 1 M lactate, demonstrated a selective oxidation of lactate to pyruvate. The combina-tion of highly selective electrochemical reactions in the LAEC and DLAFC allows for the direct storage of electrical energy in a biological liquid carrier. It is possible to complete a carbon-neutral energy cycle using the resulting energy. The LAEC/DLAFC system has the advantage of being compact with low energy consumption, as it does not require high-temperature conversion above 100 °C or the treatment of gaseous carriers.  Figure 7. An energy cycle based on a highly selective redox reaction between lactate and pyruvate obtained from biomass resources: (A) a lactic acid electrosynthesis cell (LAEC); (B) a direct lactic acid fuel cell (DLAFC). Reprinted with permission from [231]. Copyright 2023 Oxford University Press. Figure 7. An energy cycle based on a highly selective redox reaction between lactate and pyruvateobtained from biomass resources: (A) a lactic acid electrosynthesis cell (LAEC); (B) a direct lactic acidfuel cell (DLAFC). Reprinted with permission from [231]. Copyright 2023 Oxford University Press.Materials 2024, 17, 5918 11 of 27Materials 2024, 17, x FOR PEER REVIEW 11 of 27   It has been proposed that ultrathin polymer organic semiconductor films have a mul-titude of potential applications, including the development of flexible electronic devices. Nevertheless, in comparison to single crystals of low-molecular-weight organic semicon-ductors, there is considerable scope for further research in the areas of fabrication and property control. One illustrative example is the control of the electronic properties of polymer organic semiconductor films by doping. Ishii, Yamashita, and colleagues have recently published a new study which demonstrates a novel coupling between proton-coupled electron transfer reactions, which are widely employed in biochemical processes and polymer organic semiconductors (Figure 8) [232]. A p-type organic semiconductor film was immersed in an aqueous solution containing a proton-coupled electron transfer reaction redox couple (benzoquinone/hydroquinone) and a hydrophobic molecular ion. The redox potential of the former can be controlled by the proton activity (pH), which is an easily manipulable parameter. The presence of p-type doping was confirmed by meas-uring the absorption spectrum and conductivity. The efficient doping of polymer organic semiconductor films is achieved through a synergistic reaction between proton-coupled electron transfer reactions and the insertion of hydrophobic ions. The doping level was meticulously regulated within a pH-controlled aqueous solution. In other words, the Nernst equation was employed to regulate the Fermi level of the polymeric organic sem-iconductor thin film through the manipulation of proton activity. This doping method is also innovative in that it can be performed in an aqueous solution at room temperature and pressure, which renders it a method that will also be useful for industrial applications. This could prove beneficial in the creation of a platform for room-temperature semicon-ductor processes and biomolecular electronics. It will be feasible to establish a correlation between semiconductor doping and any chemical or biochemical process that can be linked with proton activity. This method is also regarded as a promising platform for bi-omolecular electronics.  Figure 8. A novel coupling between proton-coupled electron transfer reactions and polymer organic semiconductors: (top) doping mechanism; (bottom) chemical structures. Reprinted with permission from [232]. Copyright 2023 Springer-Nature. Figure 8. A novel coupling between proton-coupled electron transfer reactions and polymer organicsemiconductors: (top) doping mechanism; (bottom) chemical structures. Reprinted with permissionfrom [232]. Copyright 2023 Springer-Nature.The diverse properties of organic molecules render them an attractive option for thecreation of devices. A plethora of organic molecular structures can be synthesized throughorganic synthesis (molecular nanoarchitectonics). It is similarly important to considersupramolecular chemical processes, such as molecular association and intercalation, in or-der to control the characteristics of the devices in question. These sciences and technologieshave been the subject of study in the context of coupling fields such as organic syntheticchemistry, polymer chemistry, coordination chemistry, and supramolecular chemistry withdevice engineering. These approaches can also be unified and interpreted as molecularnanoarchitectonics. It is anticipated that this integrated approach, which transcends theboundaries of previous fields, will further advance the field of device engineering based onorganic molecules.3. Inorganic Materials NanoarchitectonicsIn addition to the organic molecules previously discussed, structurally controlled inor-ganic materials are also useful elements for device development. The nanoarchitectonicsof inorganic materials frequently permits the regulation of size, dimensions, and shape,thereby enabling the control of physical properties. This may be referred to as inorganicmaterials nanoarchitectonics in the context of device development. The following sectionwill present a number of illustrative examples.Nanoscale solid-state devices are composed of thin sheets, typically comprising only afew atomic layers, and display remarkable electronic behavior. The electronic propertiesof nano solid-state devices are markedly distinct from those of conventional solid-statedevices. In particular, the control of thickness is a crucial factor. Zhao, Fu, and colleaguesemployed an approach termed ‘thickness nanoarchitectonics’ to investigate the correlationbetween thickness and the Raman scattering and polarization characteristics of few-layerGaS nanosheets [233]. By means of a chemical vapor deposition method, three types ofGaS nanosheets with approximate thicknesses of 10, 40, and 170 nm were produced. Asthe thickness of the nanosheets increased, the intensity of the Raman scattering increasedMaterials 2024, 17, 5918 12 of 27at the edges of the nanosheets. Furthermore, the energy and polarization of the excitationphoton had a significant impact on the edge-enhanced Raman properties. Three distinct GaSnanosheet devices, comprising varying thicknesses, were fabricated and their photocurrentswere subsequently measured (Figure 9). The GaS nanosheet devices with thicknesses of 40and 170 nm exhibited positive photoresponses, despite the photocurrents being relativelylow. In contrast, the thinnest 10 nm GaS nanosheet device exhibited a substantial currenteven in the absence of light, despite its relatively weak response to light. Further studiesdemonstrated that there were differences in the spatial patterns of Raman imaging inrelation to GaS thickness, excitation light wavelength, and polarization. These findingshave implications for the potential applications of GaS and other transition metal sulfidesin fields such as photocatalysis, electrochemical hydrogen production from water splitting,energy storage, nonlinear optics, gas sensing, photodetectors, and so forth.Materials 2024, 17, x FOR PEER REVIEW 12 of 27   The diverse properties of organic molecules render them an attractive option for the creation of devices. A plethora of organic molecular structures can be synthesized through organic synthesis (molecular nanoarchitectonics). It is similarly important to consider su-pramolecular chemical processes, such as molecular association and intercalation, in order to control the characteristics of the devices in question. These sciences and technologies have been the subject of study in the context of coupling fields such as organic synthetic chemistry, polymer chemistry, coordination chemistry, and supramolecular chemistry with device engineering. These approaches can also be unified and interpreted as molec-ular nanoarchitectonics. It is anticipated that this integrated approach, which transcends the boundaries of previous fields, will further advance the field of device engineering based on organic molecules. 3. Inorganic Materials Nanoarchitectonics In addition to the organic molecules previously discussed, structurally controlled in-organic materials are also useful elements for device development. The nanoarchitectonics of inorganic materials frequently permits the regulation of size, dimensions, and shape, thereby enabling the control of physical properties. This may be referred to as inorganic materials nanoarchitectonics in the context of device development. The following section will present a number of illustrative examples. Nanoscale solid-state devices are composed of thin sheets, typically comprising only a few atomic layers, and display remarkable electronic behavior. The electronic properties of nano solid-state devices are markedly distinct from those of conventional solid-state devices. In particular, the control of thickness is a crucial factor. Zhao, Fu, and colleagues employed an approach termed ‘thickness nanoarchitectonics’ to investigate the correla-tion between thickness and the Raman scattering and polarization characteristics of few-layer GaS nanosheets [233]. By means of a chemical vapor deposition method, three types of GaS nanosheets with approximate thicknesses of 10, 40, and 170 nm were produced. As the thickness of the nanosheets increased, the intensity of the Raman scattering increased at the edges of the nanosheets. Furthermore, the energy and polarization of the excitation photon had a significant impact on the edge-enhanced Raman properties. Three distinct GaS nanosheet devices, comprising varying thicknesses, were fabricated and their photo-currents were subsequently measured (Figure 9). The GaS nanosheet devices with thick-nesses of 40 and 170 nm exhibited positive photoresponses, despite the photocurrents be-ing relatively low. In contrast, the thinnest 10 nm GaS nanosheet device exhibited a sub-stantial current even in the absence of light, despite its relatively weak response to light. Further studies demonstrated that there were differences in the spatial patterns of Raman imaging in relation to GaS thickness, excitation light wavelength, and polarization. These findings have implications for the potential applications of GaS and other transition metal sulfides in fields such as photocatalysis, electrochemical hydrogen production from water splitting, energy storage, nonlinear optics, gas sensing, photodetectors, and so forth.  Figure 9. GaS nanosheet devices comprising varying thicknesses and their photoresponsive devices. Reproduced under terms of the CC-BY license [233]. Copyright 2023 MDPI. Figure 9. GaS nanosheet devices comprising varying thicknesses and their photoresponsive devices.Reproduced under terms of the CC-BY license [233]. Copyright 2023 MDPI.Colloidal quantum dots have garnered interest due to their distinctive optoelectroniccharacteristics, which hold promise for advancement in device engineering. Furthermore,the quantum confinement effect can be enhanced by nanoarchitectonics of the core/shellstructures, thereby enabling quantum dots to be applied in light-emitting devices. Uematsu,Kuwabata, and colleagues developed a cadmium-free red-emitting quantum dot by incor-porating copper into a silver indium gallium sulfide/gallium sulfide (Ag-In-Ga-S/Ga-S)core/shell quantum dot [234]. Following the application of a Ga-S shell, the quantumdots displayed a narrow red photoluminescence spectrum. The results of experimentsconducted with varying Cu/Ag ratios indicate that the emission observed in these samplesarises from localized carriers rather than band-edge transitions. Furthermore, the researchteam investigated quantum dot-LED devices (Figure 10). In this structure, the light-emittinglayer is composed exclusively of Ag-Cu-In-Ga-S/Ga-S core/shell quantum dots, withoutthe inclusion of any additional materials to facilitate charge transport. The device displayedan electroluminescence spectrum that was almost identical to the photoluminescence ob-served in the quantum dot solution. The core/shell quantum dot LED device exhibitedhigh color purity red electroluminescence that met the BT2020 standard. The enhancedluminous efficiency and durability facilitate the practical utilization of the technology.Nanoarchitectonics studies have been conducted in which unanticipated additiveshave been observed to exert control over devices. Dey and colleagues employed a caffeineadditive-based nanoarchitectonics strategy, whereby caffeine (in the form of coffee powder)was introduced as a light absorber to methylammonium lead iodide, resulting in thedevelopment of a stable and efficient caffeine–methylammonium lead iodide perovskitesolar cell device (Figure 11) [235]. The introduction of caffeine into methylammonium leadiodide results in the production of a highly efficient and stable caffeine-based additivemethylammonium lead iodide perovskite solar cell device. The addition of caffeine tothe perovskite solar cell resulted in enhanced power conversion efficiency, short-circuitcurrent density, open-circuit voltage, fill factor, and stability when compared with the pureMaterials 2024, 17, 5918 13 of 27methylammonium lead iodide. The enhanced photovoltaic performance and stability ofcaffeine-added methylammonium lead iodide perovskite solar cells can be attributed tothe reduction in electrical resistance and the minimization of non-radiative recombinationpathways within the perovskite. The incorporation of caffeine has been demonstratedto diminish the non-radiative recombination pathways within the perovskite layer. Theincorporation of caffeine into the methylammonium lead iodide light-absorbing layer hasbeen observed to markedly enhance the electron-hole charge carriers, thereby improving thephotovoltaic performance. It is anticipated that the findings will facilitate the developmentof large-scale industrial caffeine- or similar additive-based perovskite solar cell devices.Materials 2024, 17, x FOR PEER REVIEW 13 of 27   Colloidal quantum dots have garnered interest due to their distinctive optoelectronic characteristics, which hold promise for advancement in device engineering. Furthermore, the quantum confinement effect can be enhanced by nanoarchitectonics of the core/shell structures, thereby enabling quantum dots to be applied in light-emitting devices. Uematsu, Kuwabata, and colleagues developed a cadmium-free red-emitting quantum dot by incorporating copper into a silver indium gallium sulfide/gallium sulfide (Ag-In-Ga-S/Ga-S) core/shell quantum dot [234]. Following the application of a Ga-S shell, the quantum dots displayed a narrow red photoluminescence spectrum. The results of exper-iments conducted with varying Cu/Ag ratios indicate that the emission observed in these samples arises from localized carriers rather than band-edge transitions. Furthermore, the research team investigated quantum dot-LED devices (Figure 10). In this structure, the light-emitting layer is composed exclusively of Ag-Cu-In-Ga-S/Ga-S core/shell quantum dots, without the inclusion of any additional materials to facilitate charge transport. The device displayed an electroluminescence spectrum that was almost identical to the pho-toluminescence observed in the quantum dot solution. The core/shell quantum dot LED device exhibited high color purity red electroluminescence that met the BT2020 standard. The enhanced luminous efficiency and durability facilitate the practical utilization of the technology.  Figure 10. A cadmium-free red-emitting quantum dot enabled by incorporating copper into a silver indium gallium sulfide/gallium sulfide (Ag-In-Ga-S/Ga-S) core/shell quantum dot as quantum dot-LED devices. Reprinted with permission from [234]. Copyright 2023 Oxford University Press. Nanoarchitectonics studies have been conducted in which unanticipated additives have been observed to exert control over devices. Dey and colleagues employed a caffeine additive-based nanoarchitectonics strategy, whereby caffeine (in the form of coffee Figure 10. A cadmium-free red-emitting quantum dot enabled by incorporating copper into a silverindium gallium sulfide/gallium sulfide (Ag-In-Ga-S/Ga-S) core/shell quantum dot as quantumdot-LED devices. Reprinted with permission from [234]. Copyright 2023 Oxford University Press.While not truly inorganic, materials such as wood are also applicable to the fieldof device nanoarchitectonics. The use of wood-based materials in solar steam genera-tors has gained attention in the fields of desalination and water purification due to thecost-effectiveness and potential for renewable energy sources that these generators offer.However, it should be noted that conventional solar steam generators are not always suit-able for long-term use. To this end, Li, Xu, and colleagues fabricated a bilayer compositecomprising uniformly incorporated polyaniline nanorods within a 3D mesoporous matrixof natural wood, employing a one-step in situ polymerization strategy (Figure 12) [236].The solar absorptance of polyaniline-decorated wood is exceptionally high over a broadwavelength range, due to the conjugation of coral-like polyaniline nanorods with the woodsubstrate. Furthermore, the intrinsic physical characteristics of wood impart to polyanilinewood a hydrophilic nature and the capacity to facilitate the transport of water. Further-Materials 2024, 17, 5918 14 of 27more, it displays excellent environmental and chemical resistance. The numerous alignedwood microchannels facilitate constant and rapid water transport at the air–water interface,driven by capillary forces. The polyaniline–wood composite material displays high stabilityand a high evaporation rate, indicating its potential as an optimal solar steam generator.The polyaniline–wood composite exhibits long-term buoyancy, which suggests that it hasthe potential for long-term practical application. The imminent threat of a global freshwatershortage is a direct consequence of the deterioration of global ecosystems. The generationof interfacial steam by solar means, as exemplified by this nanoarchitectonics approach tomaterial design, has the potential to provide a solution to the global water crisis.Materials 2024, 17, x FOR PEER REVIEW 14 of 27   powder) was introduced as a light absorber to methylammonium lead iodide, resulting in the development of a stable and efficient caffeine–methylammonium lead iodide per-ovskite solar cell device (Figure 11) [235]. The introduction of caffeine into methylammo-nium lead iodide results in the production of a highly efficient and stable caffeine-based additive methylammonium lead iodide perovskite solar cell device. The addition of caf-feine to the perovskite solar cell resulted in enhanced power conversion efficiency, short-circuit current density, open-circuit voltage, fill factor, and stability when compared with the pure methylammonium lead iodide. The enhanced photovoltaic performance and sta-bility of caffeine-added methylammonium lead iodide perovskite solar cells can be at-tributed to the reduction in electrical resistance and the minimization of non-radiative re-combination pathways within the perovskite. The incorporation of caffeine has been demonstrated to diminish the non-radiative recombination pathways within the perov-skite layer. The incorporation of caffeine into the methylammonium lead iodide light-ab-sorbing layer has been observed to markedly enhance the electron-hole charge carriers, thereby improving the photovoltaic performance. It is anticipated that the findings will facilitate the development of large-scale industrial caffeine- or similar additive-based per-ovskite solar cell devices.  Figure 11. Caffeine–methylammonium lead iodide perovskite solar cell device where the introduc-tion of caffeine into methylammonium lead iodide results in the production of a highly efficient and stable caffeine-based additive methylammonium lead iodide perovskite solar cell device. Reprinted with permission from [235]. Copyright 2023 Springer-Nature. While not truly inorganic, materials such as wood are also applicable to the field of device nanoarchitectonics. The use of wood-based materials in solar steam generators has gained attention in the fields of desalination and water purification due to the cost-effec-tiveness and potential for renewable energy sources that these generators offer. However, it should be noted that conventional solar steam generators are not always suitable for long-term use. To this end, Li, Xu, and colleagues fabricated a bilayer composite compris-ing uniformly incorporated polyaniline nanorods within a 3D mesoporous matrix of nat-ural wood, employing a one-step in situ polymerization strategy (Figure 12) [236]. The solar absorptance of polyaniline-decorated wood is exceptionally high over a broad Figure 11. Caffeine–methylammonium lead iodide perovskite solar cell device where the introductionof caffeine into methylammonium lead iodide results in the production of a highly efficient and stablecaffeine-based additive methylammonium lead iodide perovskite solar cell device. Reprinted withpermission from [235]. Copyright 2023 Springer-Nature.In light of the emergence of a number of novel infectious diseases, the necessity forremote monitoring of infected individuals has become paramount. This is particularlyimportant in hospitals, where infected patients must be isolated to prevent the transmissionof pathogens to medical personnel. It would be advantageous to develop wearable healthsensor devices that are capable of monitoring patients remotely. A number of infectiousdiseases can be monitored for infection status through the use of various physiologicalindicators, including abnormal body temperature, respiratory rate, and diastolic bloodpressure. As reported by Pumera and colleagues, a remote health monitoring system hasbeen developed which employs a telemedicine platform for health assessment remotely byan integrated nanoarchitectonics approach [237]. This system incorporates a stretchableasymmetric supercapacitor as a portable power source and a sensor capable of monitoringthe physical health status of humans remotely in real time (Figure 13). The system is textile-based and comprises a high-performance stretchable asymmetric supercapacitor and astrain sensor. The electrodes of the stretchable asymmetric supercapacitor and strain sensorwere composed of a composite of FePS3 and reduced graphene oxide (rGO), which werecoated on a stretchable fabric. Upon stretching the FePS3@rGO composite, a notable declinein the brightness of the red LED was observed, accompanied by a discernible alteration in itsMaterials 2024, 17, 5918 15 of 27electrical conductivity. Strain sensing is a process whereby mechanical strain is convertedinto a detectable electrical signal. Furthermore, the stretchable asymmetric supercapacitorcan be employed to power a temperature sensor positioned beneath the armpit, therebyfacilitating the monitoring of body temperature. The transmission of data from real-timemonitoring of respiration and body temperature via wireless communication to a hospitalcloud system for clinical evaluation is a viable option. The system permits patients tomonitor these health indicators without direct contact with medical personnel. The wirelessdevice developed in this study would be beneficial in situations where infected patientsrequire isolation to prevent the transmission of pathogens. Moreover, this research providesa foundation for the advancement of innovative wearable e-health monitoring systemsbased on flexible and stretchable energy storage devices.Materials 2024, 17, x FOR PEER REVIEW 15 of 27   wavelength range, due to the conjugation of coral-like polyaniline nanorods with the wood substrate. Furthermore, the intrinsic physical characteristics of wood impart to pol-yaniline wood a hydrophilic nature and the capacity to facilitate the transport of water. Furthermore, it displays excellent environmental and chemical resistance. The numerous aligned wood microchannels facilitate constant and rapid water transport at the air–water interface, driven by capillary forces. The polyaniline–wood composite material displays high stability and a high evaporation rate, indicating its potential as an optimal solar steam generator. The polyaniline–wood composite exhibits long-term buoyancy, which suggests that it has the potential for long-term practical application. The imminent threat of a global freshwater shortage is a direct consequence of the deterioration of global eco-systems. The generation of interfacial steam by solar means, as exemplified by this nano-architectonics approach to material design, has the potential to provide a solution to the global water crisis.  Figure 12. Fabricated a bilayer composite comprising uniformly incorporated polyaniline nanorods within a 3D mesoporous matrix of natural wood where the numerous aligned wood microchannels facilitate constant and rapid water transport at the air–water interface, driven by capillary forces. Reprinted with permission from [236]. Copyright 2023 Oxford University Press. In light of the emergence of a number of novel infectious diseases, the necessity for remote monitoring of infected individuals has become paramount. This is particularly im-portant in hospitals, where infected patients must be isolated to prevent the transmission of pathogens to medical personnel. It would be advantageous to develop wearable health sensor devices that are capable of monitoring patients remotely. A number of infectious diseases can be monitored for infection status through the use of various physiological indicators, including abnormal body temperature, respiratory rate, and diastolic blood pressure. As reported by Pumera and colleagues, a remote health monitoring system has been developed which employs a telemedicine platform for health assessment remotely by an integrated nanoarchitectonics approach [237]. This system incorporates a stretcha-ble asymmetric supercapacitor as a portable power source and a sensor capable of moni-toring the physical health status of humans remotely in real time (Figure 13). The system Figure 12. Fabricated a bilayer composite comprising uniformly incorporated polyaniline nanorodswithin a 3D mesoporous matrix of natural wood where the numerous aligned wood microchannelsfacilitate constant and rapid water transport at the air–water interface, driven by capillary forces.Reprinted with permission from [236]. Copyright 2023 Oxford University Press.Inorganic materials and their hybrid counterparts exhibit a range of distinctive prop-erties. In comparison to organic materials, inorganic materials possess a structure that isless flexible, yet it is relatively straightforward to precisely control the structure. The fieldof nanoarchitectonics, which encompasses techniques such as precise thickness control andcore/shell structural design, is employed in the development of devices. In comparison toorganic molecular nanoarchitectonics, which is somewhat more development-oriented, in-organic materials nanoarchitectonics demonstrates greater strengths in practical application.This is presumably due to the fact that research into inorganic materials in nanostructurecontrol has made significant advancements, resulting in the identification of specific groupsof materials that are well-suited for practical applications. This characteristic will be acrucial factor in advancing device nanoarchitectonics from the research stage to practicalapplication.Materials 2024, 17, 5918 16 of 27Materials 2024, 17, x FOR PEER REVIEW 16 of 27   is textile-based and comprises a high-performance stretchable asymmetric supercapacitor and a strain sensor. The electrodes of the stretchable asymmetric supercapacitor and strain sensor were composed of a composite of FePS3 and reduced graphene oxide (rGO), which were coated on a stretchable fabric. Upon stretching the FePS3@rGO composite, a notable decline in the brightness of the red LED was observed, accompanied by a discernible al-teration in its electrical conductivity. Strain sensing is a process whereby mechanical strain is converted into a detectable electrical signal. Furthermore, the stretchable asymmetric supercapacitor can be employed to power a temperature sensor positioned beneath the armpit, thereby facilitating the monitoring of body temperature. The transmission of data from real-time monitoring of respiration and body temperature via wireless communica-tion to a hospital cloud system for clinical evaluation is a viable option. The system per-mits patients to monitor these health indicators without direct contact with medical per-sonnel. The wireless device developed in this study would be beneficial in situations where infected patients require isolation to prevent the transmission of pathogens. More-over, this research provides a foundation for the advancement of innovative wearable e-health monitoring systems based on flexible and stretchable energy storage devices.  Figure 13. A remote health monitoring system based on a telemedicine platform for remote health assessment by an integrated nanoarchitectonics approach in which the electrodes of the stretchable asymmetric supercapacitor and strain sensor were composed of a composite of FePS3 and reduced graphene oxide coated on a stretchable fabric. Reproduced under terms of the CC-BY license [237]. Copyright 2022 Springer-Nature. Inorganic materials and their hybrid counterparts exhibit a range of distinctive prop-erties. In comparison to organic materials, inorganic materials possess a structure that is less flexible, yet it is relatively straightforward to precisely control the structure. The field of nanoarchitectonics, which encompasses techniques such as precise thickness control and core/shell structural design, is employed in the development of devices. In compari-son to organic molecular nanoarchitectonics, which is somewhat more development-ori-ented, inorganic materials nanoarchitectonics demonstrates greater strengths in practical application. This is presumably due to the fact that research into inorganic materials in nanostructure control has made significant advancements, resulting in the identification of specific groups of materials that are well-suited for practical applications. This charac-teristic will be a crucial factor in advancing device nanoarchitectonics from the research stage to practical application.   Figure 13. A remote health monitoring system based on a telemedicine platform for remote healthassessment by an integrated nanoarchitectonics approach in which the electrodes of the stretchableasymmetric supercapacitor and strain sensor were composed of a composite of FePS3 and reducedgraphene oxide coated on a stretchable fabric. Reproduced under terms of the CC-BY license [237].Copyright 2022 Springer-Nature.4. Conclusions and Future PerspectivesAs previously stated in the introduction, it is crucial to consider the role of nanotech-nology in the evolution towards nanoarchitectonics, particularly in relation to its impacton device hardware applications. This represents a solution to the well-known problem ofcombining top-down and bottom-up approaches in the development of functional systems.The microfabrication techniques that are prominent in nanotechnology are an example ofa top-down approach, whereas device nanoarchitectonics, which involves the assemblyof functional materials from atoms and molecules, is a powerful bottom-up approach.Device nanoarchitectonics will represent the convergence of top-down and bottom-upapproaches. It will serve as an illustrative example of the convergence of nanotechnologyand materials science.In this review, components are roughly divided into organic compounds and inorganicmaterials. Although the fundamental parts of device functional architecture are almost thesame, each has its own characteristics. For example, many devices that exhibit optical andelectronic functions are heavily dependent on the properties of the molecules that performtheir functions. In other words, the development of functional molecules is a major key.Organic molecules have diverse properties, and their characteristics are attractive for devicecreation. The structures of organic molecules are diverse, and there are various controlelements such as π-conjugated structures, chemical structures of complex ligands, sterichindrance effects, molecular stacking, isomerization and color changes due to externalstimuli, control of selective redox reactions, and doping control of organic semiconductorsby electron transfer reactions, to name just a few. The structures of organic molecules can becreated in a variety of ways through organic synthesis (molecular architectonics). In addi-tion, supramolecular chemical processes such as molecular association and intercalation arealso important for controlling device characteristics. On the other hand, nanoarchitectonicsof inorganic materials often allows control of size, dimension, and shape, and the associatedphysical properties can also be controlled. Among the examples of structural elementsgiven here, precise thickness control, core/shell structure, additive control, environmentaland chemical resistance, and composite materials for multifunctional devices are recog-nized. Generally speaking, nano-inorganic materials are characterized by the ease of precisestructural control. In addition, there are specific material groups suitable for practical use,Materials 2024, 17, 5918 17 of 27such as nanoparticles and graphene. Therefore, inorganic materials nanoarchitectonics isalso closer to the practical stage. Of course, detailed examinations and confirmations ofactual performances and functions of the materials and devices prepared with nanoarchitec-tonics concepts are important. In particular, attention must be given to concrete parameters,temperature conditions, pressure conditions, and the selection of materials to ensure thereproducibility, durability, stability, effectiveness, environmental impacts, sustainability,chemical availability, and cost-benefits upon comparisons with the control matters of ex-isting technologies, materials, and real devices with detailed statistical analyses. Theseinvestigations will practically prove true the meanings of the nanoarchitectonics approach.In the field of device nanoarchitectonics, there are notable distinctions between or-ganic molecules and inorganic materials. However, the fundamental methodology ofconstructing functional devices using nanounits is largely similar. Rather than developingthese large component elements independently, it would be more beneficial to hybridizeand integrate them in order to construct more functional devices. The properties of thefunctional materials that are to be incorporated as components are diverse and somewhatidiosyncratic. Furthermore, the anticipated functional outcome is also highly variable.Therefore, it is anticipated that a multitude of functions will be expressed within the samedevice. It may prove challenging for humans to process this diversity-based approach,given past experience and existing achievements. In order to develop functional devicesin an efficient and innovative manner, it will be necessary to utilize the capabilities ofartificial intelligence. It is evident that machine learning [238–240] and materials informat-ics [241–243] have made significant contributions to materials sciences and other relatedfields. Additionally, there are publications that address the integration of nanoarchitec-tonics and artificial intelligence [244,245]. In the context of device development, there isa substantial accumulation of data that can be utilized as a basis for artificial intelligence,given that the materials employed, the structure, the function, and the output are all subjectto rigorous examination. The further development of device nanoarchitectonics will becontingent upon the introduction of artificial intelligence. Furthermore, there is a pressingneed for the advancement of device nanoarchitectonics into the realm of practical devices.At that juncture, it will be increasingly advantageous to integrate it with microfabricationtechnology oriented towards mass production. This indicates that the integration of bottom-up science and top-down technology will be a highly beneficial approach. The adventof artificial intelligence will facilitate this process. Nanoarchitectonics approaches withartificial intelligence may even provide the potential for long-term practical applicationswithout providing sufficient empirical data or tests that could substantiate durability andresilience over extended periods. In particular, such considerations have to be taken withthe viewpoint that the materials used are environmentally friendly even though it lacks alife-cycle analysis or comparative assessment against conventional materials. The nanoar-chitectonics approach effectively integrates devices across various applications as seen inpossible examples of remote health monitoring (for the practical clinical effects see thecorresponding original papers). 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MDPI and/or the editor(s) disclaim responsibility for any injury topeople or property resulting from any ideas, methods, instructions or products referred to in the content.https://doi.org/10.1007/s10854-023-11569-2https://doi.org/10.1246/bcsj.20230145https://doi.org/10.1038/s41528-022-00208-1https://doi.org/10.1016/j.mtphys.2023.100971https://doi.org/10.1103/PhysRevMaterials.7.034410https://doi.org/10.1093/bulcsj/uoae090https://doi.org/10.1557/mrs2006.223https://doi.org/10.1038/s41524-017-0056-5https://doi.org/10.1007/s10853-024-09379-whttps://doi.org/10.1002/adma.202107212https://www.ncbi.nlm.nih.gov/pubmed/34637159https://doi.org/10.1007/s11051-022-05535-y Introduction  Organic Molecular Nanoarchitectonics  Inorganic Materials Nanoarchitectonics  Conclusions and Future Perspectives  References